P 2 S 5 Reactive Flux Method for the Rapid Synthesis of Mono- and Bimetallic 2D Thiophosphates M 2–x M′ x P 2 S 6
- Award ID(s):
- 1929356
- PAR ID:
- 10280293
- Date Published:
- Journal Name:
- Inorganic Chemistry
- Volume:
- 60
- Issue:
- 6
- ISSN:
- 0020-1669
- Page Range / eLocation ID:
- 3502 to 3513
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Antiferromagnetic van der Waals‐typeM2P2X6compounds provide a versatile material platform for studying 2D magnetism and relevant phenomena. Establishing ferromagnetism in 2D materials is technologically valuable. Though magnetism is generally tunable via a chemical way, it is challenging to induce ferromagnetism with isovalent chalcogen and bimetallic substitutions inM2P2X6. Here, we report co‐substitution of Cu1+and Cr3+for Ni2+in Ni2P2S6, creating CuxNi2(1‐x)CrxP2S6medium‐entropy alloys spanning a full substitution range (x= 0 to 1). Such substitution strategy leads to a unique evolution in crystal structure and magnetic phases that are distinct from traditional isovalent bimetallic doping, with Cu and Cr co‐substitution enhancing ferromagnetic correlations and generating a weak ferromagnetic phase in intermediate compositions. This aliovalent substitution strategy offers a universal approach for tuning layered magnetism in antiferromagnetic systems, which along with the potential for light‐matter interaction and high‐temperature ferroelectricity, can enable multifunctional device applications.more » « less
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